The goal of the chemistry described herein is to expand the utility of the already versatile eta6(arene)Cr(CO)3 compounds in organic synthesis by examining their reactivity with ambiphilic reagents such as sulfur and related ylides as well as enolate ions of alpha-halo esters, amides and nitriles. This chemistry is expected to provide access to a number of useful classes of molecules such as substituted norcaradienes and cycloheptatrienes as well as [4.1.0] bicycloheptenones. The methodology should prove complementary to the existing methods which exist for the preparation of such molecules, which would undoubtedly prove useful in a variety of theoretical and total synthetic studies. Ultimately, such methodology might be accomplished asymmetrically thus increasing its usefulness even further.